B4 - Multiscale Modeling of the Oxidative Removal of Pollutants


This project aims at a theoretical description of the oxidative removal of pollutants over noble metal based catalysts by a multiscale approach using DFT calculations that form the basis of kinetic modeling of reactor models. As starting point we consider investigations of CO and CH4 oxidation over supported Pt and Pd-based catalysts. Central questions relate to the identification of the active site for the various types of materials investigated and the corresponding reaction mechanism at the atomic-scale. Using the kinetics derived from the DFT calculations an elementary-step-based microkinetic model will be developed for fixed bed/plug flow (1D) and channel (2D) reactor models.

Project-related publications by participating researchers

Project- and subject-related list of publications

S. D. Angeli, S. Gossler, S. Lichtenberg, G. Kass, A. Agrawal, M. Valerius, K.-P. Kinzel, O. Deutschmann, Reduction of CO2 Emission from Offgases of Steel Industry by Dry Reforming of Methane. Angew. Chemie Int. Ed. 2021, 60 (21), 1185211857.

DOI: 10.1002/anie.202100577

J. Chawla, S. Schardt, S. Angeli, P. Lott, S. Tischer, L. Maier, O. Deutschmann, Oxidative Coupling of Methane over Pt/Al2O3 at High Temperature: Multiscale Modeling of the Catalytic Monolith. Catalysts 2022, 12 (2), 189.

DOI: 10.3390/catal12020189

R. Chacko, K. Keller, S. Tischer, A. B. Shirsath, P. Lott, S. Angeli, O. Deutschmann, Automating the Optimization of Catalytic Reaction Mechanism Parameters Using Basin-Hopping: A Proof of Concept. J. Phys. Chem. C 2022, 127 (16), 76287639.

DOI: 10.1021/acs.jpcc.2c08179

J. Chawla, S. Schardt, P. Lott, S. Angeli, S. Tischer, L. Maier, O. Deutschmann, Detailed Kinetic Modeling of Catalytic Oxidative Coupling of Methane. Chem. Eng. J. 2024, 148719.

DOI: 10.1016/j.cej.2024.148719

B. Kreitz, P. Lott, J. Bae, K. Blöndal, S. Angeli, Z. W. Ulissi, F. Studt, C. F. Goldsmith, O. Deutschmann, Detailed Microkinetics for the Oxidation of Exhaust Gas Emissions through Automated Mechanism Generation. ACS Catal. 2022, 12 (18), 1113711151.

DOI: 10.1021/acscatal.2c03378

B. Kreitz, P. Lott, F. Studt, A. J. Medford, O. Deutschmann, C. F. Goldsmith, Automated Generation of Microkinetics for Heterogeneously Catalyzed Reactions Considering Correlated Uncertainties**. Angew. Chemie - Int. Ed. 2023.

DOI: 10.1002/anie.202306514

F. Maurer, J. Jelic, J. Wang, A. Gänzler, P. Dolcet, C. Wöll, Y. Wang, F. Studt, M. Casapu, J.-D. Grunwaldt, Tracking the Formation, Fate and Consequence for Catalytic Activity of Pt Single Sites on CeO2. Nat. Catal. 2020, 3 (10), 824833.

DOI: 10.1038/s41929-020-00508-7

F. Maurer, A. Beck, J. Jelic, W. Wang, S. Mangold, M. Stehle, D. Wang, P. Dolcet, A. M. Gänzler, C. Kübel, F. Studt, M. Casapu, J.-D. Grunwaldt, Surface Noble Metal Concentration on Ceria as a Key Descriptor for Efficient Catalytic CO Oxidation. ACS Catal. 2022, 12 (4), 24732486.

DOI: 10.1021/acscatal.1c04565

B. B. Sarma, J. Jelic, D. Neukum, D. E. Doronkin, X. Huang, F. Studt, J.-D. Grunwaldt, Tracking and Understanding Dynamics of Atoms and Clusters of Late Transition Metals with In-Situ DRIFT and XAS Spectroscopy Assisted by DFT. J. Phys. Chem. C 2023, 127 (6), 30323046.

DOI: 10.1021/acs.jpcc.2c07263

C. Yang, Y. Cao, P. N. Plessow, J. Wang, A. Nefedov, S. Heissler, F. Studt, Y. Wang, H. Idriss, T. G. Mayerhöfer, C. Wöll, N2O Adsorption and Photochemistry on Ceria Surfaces. J. Phys. Chem. C 2022, 126 (4), 22532263.

DOI: 10.1021/acs.jpcc.1c10181